Document Detail

Asymmetric collapse in biomimetic complex coacervates revealed by local polymer and water dynamics.
MedLine Citation:
PMID:  23540713     Owner:  NLM     Status:  MEDLINE    
Complex coacervation is a phenomenon characterized by the association of oppositely charged polyelectrolytes into micrometer-scale liquid condensates. This process is the purported first step in the formation of underwater adhesives by sessile marine organisms, as well as the process harnessed for the formation of new synthetic and protein-based contemporary materials. Efforts to understand the physical nature of complex coacervates are important for developing robust adhesives, injectable materials, or novel drug delivery vehicles for biomedical applications; however, their internal fluidity necessitates the use of in situ characterization strategies of their local dynamic properties, capabilities not offered by conventional techniques such as X-ray scattering, microscopy, or bulk rheological measurements. Herein, we employ the novel magnetic resonance technique Overhauser dynamic nuclear polarization enhanced nuclear magnetic resonance (DNP), together with electron paramagnetic resonance (EPR) line shape analysis, to concurrently quantify local molecular and hydration dynamics, with species- and site-specificity. We observe striking differences in the structure and dynamics of the protein-based biomimetic complex coacervates from their synthetic analogues, which is an asymmetric collapse of the polyelectrolyte constituents. From this study we suggest charge heterogeneity within a given polyelectrolyte chain to be an important parameter by which the internal structure of complex coacervates may be tuned. Acquiring molecular-level insight to the internal structure and dynamics of dynamic polymer complexes in water through the in situ characterization of site- and species-specific local polymer and hydration dynamics should be a promising general approach that has not been widely employed for materials characterization.
Julia H Ortony; Dong Soo Hwang; John M Franck; J Herbert Waite; Songi Han
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Publication Detail:
Type:  Journal Article; Research Support, N.I.H., Extramural; Research Support, Non-U.S. Gov't; Research Support, U.S. Gov't, Non-P.H.S.     Date:  2013-04-19
Journal Detail:
Title:  Biomacromolecules     Volume:  14     ISSN:  1526-4602     ISO Abbreviation:  Biomacromolecules     Publication Date:  2013 May 
Date Detail:
Created Date:  2013-05-13     Completed Date:  2013-12-16     Revised Date:  2014-08-03    
Medline Journal Info:
Nlm Unique ID:  100892849     Medline TA:  Biomacromolecules     Country:  United States    
Other Details:
Languages:  eng     Pagination:  1395-402     Citation Subset:  IM    
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MeSH Terms
Amino Acid Sequence
Biomimetic Materials / chemistry*
Electron Spin Resonance Spectroscopy
Hyaluronic Acid / chemistry*
Hydrogen-Ion Concentration
Magnetic Resonance Spectroscopy
Molecular Sequence Data
Mytilus edulis / chemistry
Recombinant Proteins / chemistry
Spin Labels
Static Electricity
Water / chemistry*
Grant Support
Reg. No./Substance:
0/Recombinant Proteins; 0/Spin Labels; 059QF0KO0R/Water; 9004-61-9/Hyaluronic Acid

From MEDLINE®/PubMed®, a database of the U.S. National Library of Medicine

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